Reaction Mechanism and Kinetics for CO Reduction on Nickel Single Atom Catalysts from Quantum Mechanics

Overview

Journal Nat Commun

Specialty Biology

Date 2020 May 9

PMID 32382033

Citations 24

Authors

Md Delowar Hossain

Yufeng Huang

Ted H Yu

William A Goddard Iii

Zhengtang Luo

Affiliations

Soon will be listed here.

Abstract

Experiments have shown that graphene-supported Ni-single atom catalysts (Ni-SACs) provide a promising strategy for the electrochemical reduction of CO to CO, but the nature of the Ni sites (Ni-NC, Ni-NC, Ni-N) in Ni-SACs has not been determined experimentally. Here, we apply the recently developed grand canonical potential kinetics (GCP-K) formulation of quantum mechanics to predict the kinetics as a function of applied potential (U) to determine faradic efficiency, turn over frequency, and Tafel slope for CO and H production for all three sites. We predict an onset potential (at 10 mA cm) U = -0.84 V (vs. RHE) for Ni-NC site and U = -0.92 V for Ni-NC site in agreement with experiments, and U = -1.03 V for Ni-N. We predict that the highest current is for Ni-N, leading to 700 mA cm at U = -1.12 V. To help determine the actual sites in the experiments, we predict the XPS binding energy shift and CO vibrational frequency for each site.

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